TY - JOUR
T1 - Unveiling the promoting mechanism of Mo on the performance of CuCeOx catalyst for simultaneously NH3-SCR denitration and CO oxidation under oxygen-rich conditions
AU - Shen, Zhenghua
AU - Xing, Xiangdong
AU - She, Yuan
AU - Guo, Penghui
AU - Ren, Shan
AU - Niu, Wenkang
AU - Li, Jixuan
AU - Li, Huizi
AU - Meng, Hao
N1 - Publisher Copyright:
© 2024 Elsevier B.V.
PY - 2025/3/1
Y1 - 2025/3/1
N2 - NOx and CO coexisted in numerous actual industrial flue gases. The simultaneous removal of NOx and CO had great potential for application but remained still a challenge. Herein, a series of Mo-modified CuCeOx catalyst was developed to simultaneously achieve NH3-SCR denitration and CO oxidation. The results indicated that the CCM3 catalyst displayed the optimal performance with 91.2 % NOx conversion and 100 % CO conversion as well as excellent long-time stability and SO2 or/and H2O tolerance at 225 ℃. It was found that the strong interaction between Cu, Ce and Mo oxides resulted in the particles highly dispersed with smaller size on catalyst surface, which could provide abundant active sites to decreasing the competitive adsorption among reactive gases. Furthermore, the Mo modification promoted the production of more oxygen vacancies, Ce3+ and Oα species, which facilitated the redox recycle and the generation of intermediates. Moreover, the H2-TPR and NH3/CO/O2-TPD analysis illustrated that the reducibility and the capacity for reaction gas adsorption and activation were enhanced, which improved low-temperature activity. The in situ DRIFTS experiment revealed that the E-R and L-H mechanism were existed in NH3-SCR process on CC and CCM3 catalysts. What's more, the stronger acidity and strengthened E-R mechanism on CCM3 catalyst hindered the adsorption of SO2 and weakened the inhibition effect of competitive adsorption among SO2 and NO. Additionally, both surface lattice oxygen and chemisorbed oxygen could react with Cu+–CO species to produce CO2, the pathway obeyed L-H and MvK mechanism. This work may provide a novel strategy for the treatment of CO and NOx pollutants in industrial flue gas.
AB - NOx and CO coexisted in numerous actual industrial flue gases. The simultaneous removal of NOx and CO had great potential for application but remained still a challenge. Herein, a series of Mo-modified CuCeOx catalyst was developed to simultaneously achieve NH3-SCR denitration and CO oxidation. The results indicated that the CCM3 catalyst displayed the optimal performance with 91.2 % NOx conversion and 100 % CO conversion as well as excellent long-time stability and SO2 or/and H2O tolerance at 225 ℃. It was found that the strong interaction between Cu, Ce and Mo oxides resulted in the particles highly dispersed with smaller size on catalyst surface, which could provide abundant active sites to decreasing the competitive adsorption among reactive gases. Furthermore, the Mo modification promoted the production of more oxygen vacancies, Ce3+ and Oα species, which facilitated the redox recycle and the generation of intermediates. Moreover, the H2-TPR and NH3/CO/O2-TPD analysis illustrated that the reducibility and the capacity for reaction gas adsorption and activation were enhanced, which improved low-temperature activity. The in situ DRIFTS experiment revealed that the E-R and L-H mechanism were existed in NH3-SCR process on CC and CCM3 catalysts. What's more, the stronger acidity and strengthened E-R mechanism on CCM3 catalyst hindered the adsorption of SO2 and weakened the inhibition effect of competitive adsorption among SO2 and NO. Additionally, both surface lattice oxygen and chemisorbed oxygen could react with Cu+–CO species to produce CO2, the pathway obeyed L-H and MvK mechanism. This work may provide a novel strategy for the treatment of CO and NOx pollutants in industrial flue gas.
KW - CO oxidation
KW - CuCeO catalyst
KW - Mo species
KW - NH-SCR
KW - Simultaneous removal
UR - https://www.scopus.com/pages/publications/85204056776
U2 - 10.1016/j.seppur.2024.129561
DO - 10.1016/j.seppur.2024.129561
M3 - 文章
AN - SCOPUS:85204056776
SN - 1383-5866
VL - 355
JO - Separation and Purification Technology
JF - Separation and Purification Technology
M1 - 129561
ER -